Title

Author

Document Type

Dissertation

Date of Degree

2012

Degree Name

PhD (Doctor of Philosophy)

Degree In

Chemical and Biochemical Engineering

First Advisor

Gregory R. Carmichael

Abstract

The impacts of transported and locally-produced pollutants on western US air quality during summer 2008 are studied using the multi-scale Sulfur Transport and Deposition Modeling system. Transported background (TBG) is an indicator of the influences from extra-regional emissions or the lower stratosphere. The magnitude of TBG is expected to increase as the emissions from international sources grow. This trend is especially important in the context of US air quality standards, which tend to become more stringent to protect human health and ecosystems. Forward sensitivity simulations in which the model boundary conditions and emissions are perturbed show that TBG strongly and extensively affect western US surface ozone (more than half of the total), compared to other contributors to background ozone (North American, NA, biomass burning, BB and biogenic emissions), and the impacts differ among various geographical regions and land types. The stratospheric ozone impacts are weak. The TBG ozone contributes most to western US ozone among all TBG species, and TBG peroxyacetyl nitrate is the most important species among ozone precursors. Compared to monthly mean 8-hour daily maximum ozone, the secondary standard metric "W126 monthly index" shows larger responses to TBG perturbations and stronger non-linearity to the size of perturbations. Overall the model-estimated TBG impacts negatively correlate to the vertical resolution and positively correlate to the horizontal resolution. The estimated TBG impacts weakly depend on the magnitude of uncertainties in the US anthropogenic emissions. The transport/subsidence processes that link airmasses aloft with the surface pollution level are analyzed by trajectories, time-lag correlation and adjoint sensitivity analyses. Various types of observations are used to identify source regions and transport processes, and to improve model prediction using the four-dimensional variational data assimilation during a long-range transport episode.

The sectoral and geographical contributions to summertime US black carbon (BC) distributions are studied. NA emissions heavily (>70%) affect the BC levels from the surface to 5 km, while non-NA plumes compose more than half of the BC above 5 km. NA and non-NA BB, NA transportation and non-NA residential emissions are the major contributing sectors. Aircraft measurements during the California phase of the Arctic Research of the Composition of the Troposphere from Aircraft andSatellites (ARCTAS-CARB) field campaign show that BC/(organic matter + nitrate + sulfate) mass ratios fairly well represent BC's warming potential over southern California, which can be approximated by BC/(organic matter + sulfate) and BC/sulfate for plumes affected and unaffected by fires, respectively. The responses of BC/(organic matter + sulfate) and BC/sulfate to removing each emission sector indicate that mitigating NA transportation emissions has the highest potential for regional air quality and climate co-benefits. Contributions from NA BB and extra-regional emissions differ for summer and spring (April 2008).

Keywords

atmospheric modeling, pollution transport, source attribution, western US air quality